CN105651837B - Microelectrode system and preparation method thereof, electrochemical sensor - Google Patents
Microelectrode system and preparation method thereof, electrochemical sensor Download PDFInfo
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- CN105651837B CN105651837B CN201511021604.5A CN201511021604A CN105651837B CN 105651837 B CN105651837 B CN 105651837B CN 201511021604 A CN201511021604 A CN 201511021604A CN 105651837 B CN105651837 B CN 105651837B
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/28—Electrolytic cell components
- G01N27/30—Electrodes, e.g. test electrodes; Half-cells
Abstract
The invention discloses the microelectrode systems of three kinds of Microelectrode array architectures, it is that a kind of two-dimentional interdigital structure, a kind of spiral interdigital structure and a kind of spiral intersect the microelectrode system of interdigital structure, electrochemical sensor and preparation method thereof respectively, to provide continuous field distribution, response performance is improved.
Description
Technical field
The present invention relates to technical field of electrochemical detection more particularly to a kind of microelectrode system and preparation method thereof, electrifications
Learn sensor.
Background technology
Electrochemical sensor and detecting system since to have the advantages that be easy to micromation, high sensitivity, specificity good for it,
Biology, medicine, food security, environmental monitoring, military affairs, medicine and other fields suffer from important application value.
Critical component, that is, electrode system of electrochemical sensor.Compared to conventional electrodes, ultramicroelectrode has the speed of response
Soon, the electrochemical properties that current strength is small while current density is big, coefficient of mass transfer is big.
Ultra-micro array electrode refers to by the single electrode of multiple ultramicroelectrode collection formed appearance bundled together, electric current
It is the summation of each single ultramicroelectrode electric current.This electrode had not only maintained the characteristic of original single ultramicroelectrode, but also can obtain
Larger current strength is obtained, the sensitivity of electroanalysis is improved.Wherein, interdigitation micro-strip electrode array has generation-collection effect,
The sensitivity of detection can be improved, realize low concentration detection.
But the reduction of the size due to electrode, edge effect and point effect significantly increase, the electrode system for being it is steady
Qualitative variation.How while electrode system is miniaturized, sensitivity and the stability of detection are improved as far as possible, are realized more preferable
Detection performance, be increasingly becoming research hotspot.
In the implementation of the present invention, applicants have appreciated that technological deficiency of the existing technology：It is super using interdigitation
The electrode of the electrode system generation of microelectrode array is simultaneously inhomogenous, therefore the response stability of sample to be tested can be affected.
Invention content
(1) technical problems to be solved
In order to solve drawbacks described above, the present invention provides the microelectrode systems of three kinds of Microelectrode array architectures, are one respectively
The two-dimentional interdigital structure of kind, a kind of spiral interdigital structure and a kind of spiral intersect the microelectrode system of interdigital structure, electrochemical sensing
Device and preparation method thereof improves response performance to provide continuous field distribution.
(2) technical solution
According to an aspect of the invention, there is provided a kind of microelectrode system comprising：Dielectric substrate；And dielectric substrate
On the first, second two electrodes, constitute a pair of electrodes, single electrode is comb arrays structure, insulated from each other, first and second
Electrode is mutually nested.
According to another aspect of the present invention, a kind of microelectrode system is provided comprising：Dielectric substrate；Dielectric substrate
On spiral interdigital electrode constitute a pair of electrodes for the first, second two electrodes, single electrode is spiral unilateral side pectination knot
Structure, insulated from each other, the two is mutually nested.
According to another aspect of the present invention, a kind of microelectrode system is provided comprising：Dielectric substrate；Dielectric substrate
On spiral intersect interdigital electrode, for the first, second two electrodes, constitute a pair of electrodes, single electrode is spiral bilateral comb
Shape structure, insulated from each other, the two is mutually nested.
According to another aspect of the present invention, a kind of electrochemical sensor is provided, which includes above-mentioned
Microelectrode system.
According to another aspect of the present invention, a kind of method preparing microelectrode system, including step are provided：In cleaning
Dielectric substrate on spin coating photoresist；Photoetching is carried out to the photoresist of institute's spin coating, exposes microelectrode pattern；Using sputtering or steam
The method of plating forms the microelectrode pattern of microelectrode system proposed by the present invention on an insulating substrate；Remove remaining photoresist.
(3) advantageous effect
The microelectrode system that present invention two dimension interdigital structure, spiral interdigital structure, spiral intersect interdigital structure has one respectively
Microelectrode is constituted in micron, symmetrical nested stereo electrod to size, is had the advantages that：1) two dimension in the present invention
The microelectrode system that interdigital structure, spiral interdigital structure, spiral intersect interdigital structure is capable of providing continuous field distribution, improves
The stability responded in Electrochemical Detection；2) three kinds of microelectrode systems in the present invention, the size of electrode is in micron or Asia
Micron order, the electric field overwhelming majority concentrate on electrode surface so that electrode exchanges rapidly, is effectively utilized the amplification of microelectrode array
Effect improves sensitivity.3) the two-dimentional interdigital structure in the present invention, spiral interdigital structure, spiral intersect the micro- electricity of interdigital structure
Electrode systems can provide uniform electric field in electrode two-dimensional surface so that entire microelectrode system is more stablized.
Description of the drawings
Fig. 1 is the structural schematic diagram according to the two-dimentional interdigital structure microelectrode system of first embodiment of the invention；
Fig. 2 is the structural schematic diagram according to the spiral interdigital structure microelectrode system of second embodiment of the invention；
Fig. 3 is the structural schematic diagram for intersecting interdigital structure microelectrode system according to the spiral of third embodiment of the invention；
Fig. 4 is the schematic diagram of microelectrode system controlling Preparation Method of the present invention.
Specific implementation mode
To make the objectives, technical solutions, and advantages of the present invention clearer, below in conjunction with specific embodiment, and reference
Attached drawing, the present invention is described in more detail.
According to an aspect of the present invention, a kind of microelectrode system is proposed.Fig. 1 is the first embodiment of the microelectrode system
Structural schematic diagram.
Referring to Fig.1, which is two-dimentional interdigital structure, including：Dielectric substrate；Two dimension in dielectric substrate is intersected
It is interdigital, it is two electrodes, single electrode is comb arrays structure, insulated from each other, and mutually nested formation crossed structure.
Fig. 2 is the structural schematic diagram of the second embodiment of the microelectrode system.
With reference to Fig. 2, which is spiral interdigital structure, including：Dielectric substrate；Spiral in dielectric substrate is interdigital
Electrode is two electrodes, and single electrode is spiral pectinate texture, insulated from each other and mutually nested at spiral interdigital structure.
Fig. 3 is the structural schematic diagram of the 3rd embodiment of the microelectrode system.
With reference to Fig. 3, which is spiral intersection interdigital structure, including：Dielectric substrate；Spiral in dielectric substrate
Intersect interdigital electrode, is two electrodes, single electrode is spiral pectinate texture, insulated from each other, and mutually nested is handed at spiral
Pitch structure.
In the microelectrode system of the present invention, insulating layer is preferably silicon dioxide layer, and the thickness of the silicon dioxide layer is between 1
Micron is between 10 microns.The material of microelectrode is sensitive conductive material, it is preferable that the sensitive conductive material is gold, platinum and silver.
In addition, in order to ensure that sensitive conductive material and dielectric substrate effectively bond, it is preferable that in vapor deposition, sputtering or the sensitive gold of deposition
Before belonging to material, it is initially formed one layer of bonding metal layer.By taking gold as an example, bonding metal layer choosing selects chromium or titanium, the thickness of bonding metal layer
Degree is between 10 nanometers to 50 nanometers.
Pectination microelectrode is mutually nested, and broach width and mutual broach spacing closely are all between 10 nanometers to 20 microns
Between, the height of broach is between 50 nanometers to 1 micron.In the microelectrode system of the present embodiment, spacing only has between electrode
Micron order or nanoscale, electrode concentrate on reaction surface so that electron exchange is rapid, is effectively utilized putting for microelectrode array
Big effect, to improve the sensitivity of electrode system.Preferably, broach width and mutual broach spacing closely are all between 5
Micron is between 20 microns, and height is between 50 nanometers to 300 nanometers.
The microelectrode system of the present invention is capable of providing continuous field distribution, is different from general interdigital microstrip array electrode
Inhomogenous field distribution, to provide more stable response performance.Preferably, one in the microelectrode system of different structure
Include the terminals of connection to electrode, the terminals are for the connection with external detection equipment.
According to another aspect of the present invention, it is also proposed that a kind of electrochemical sensor, the electrochemical sensor include the present invention
Any microelectrode system in the above-mentioned three kinds of structures proposed.
In accordance with a further aspect of the present invention, it is also proposed that a kind of microelectrode system controlling Preparation Method, of the invention three kinds of microelectrodes
System is made of dielectric substrate and a pair of of size in sub-micron or micron-sized electrode, and two electrodes are mutually nested, using half
Prepared by semiconductor process, specific preparation method includes：Step S01 gets out clean dielectric substrate.Step S02, in the exhausted of cleaning
Edge substrate spin coating photoresist；Step S03 carries out photoetching to the photoresist of revolved figure, exposes target pattern；Step S04 and step
S05 respectively sputters adhesive and sensitive metal material using the technique of magnetron sputtering or vapor deposition or steams to the substrate exposed
On, it forms two-dimentional interdigital structure, spiral interdigital structure or spiral and intersects interdigital figure；Step S06 removes remaining photoetching
Glue.
According to a specific example of this method, the preferred quartz substrate of dielectric substrate.In quartz substrate, vapor deposition two dimension is interdigital
Structure microelectrode, electrode sensitive metal material are gold, by the fixation of subsequent biosensor, are formed and are examined to alpha-fetoprotein
The two-dimentional interdigital structure microelectrode system of survey.In step S02, the spin coating photoresist in clean quartz substrate, thickness is 4 micro-
Rice；In step S03, ultraviolet light is lithographically formed microelectrode pattern, the mould as microelectrode；In step S04 and step S05,
30nm chromium and 200nm gold are sputtered in quartz substrate after photoetching, wherein layer gold is as sensitive metal layer, and layers of chrome is as layer gold and stone
Adhesive layer between English substrate；Photoresist mould is removed with acetone soak in step S06, retains the two dimension being made of chromium, gold
The microelectrode system of interdigital structure；In step S07, when the interdigital microelectrode system of two dimension prepared using above-mentioned technique is tested
When, the antibody of alpha-fetoprotein is fixed in gold electrode surfaces using the method assembled in vain, is formed and the two dimension that alpha-fetoprotein detects is pitched
Refer to the impedance biological sensing system of microelectrode.
Particular embodiments described above has carried out further in detail the purpose of the present invention, technical solution and advantageous effect
Describe in detail bright, it should be understood that the above is only a specific embodiment of the present invention, is not intended to restrict the invention, it is all
Within the spirit and principles in the present invention, any modification, equivalent substitution, improvement and etc. done should be included in the protection of the present invention
Within the scope of.
Claims (10)
1. a kind of microelectrode system comprising：Dielectric substrate；Spiral interdigital electrode in dielectric substrate is first, second liang
A electrode constitutes a pair of electrodes, and single electrode is spiral unilateral side pectinate texture, and insulated from each other, the two is mutually nested；Wherein, institute
The first electrode and second electrode stated are in three-dimensional structure, and the spacing between width and adjacent electrode is micro- between 200 nanometers to 20
Between rice, highly between 20 nanometers to 1 micron.
2. a kind of microelectrode system comprising：Dielectric substrate；Spiral in dielectric substrate intersects interdigital electrode, is first, the
2 two electrodes constitute a pair of electrodes, and single electrode is spiral bilateral pectinate texture, and insulated from each other, the two is mutually nested；Its
In, the first electrode and second electrode are in three-dimensional structure, the spacing between width and adjacent electrode between 200 nanometers extremely
Between 20 microns, highly between 20 nanometers to 1 micron.
3. microelectrode system according to claim 1 or 2, which is characterized in that first, second electrode all extends to company
The terminals connect, the terminals are for the connection with external detection equipment.
4. microelectrode system according to claim 1, which is characterized in that the first, second electrode is that involute spiral is unilateral
Pectinate texture.
5. microelectrode system according to claim 2, which is characterized in that the first, second electrode is involute spiral bilateral
Pectinate texture.
6. microelectrode system according to claim 1 or 2, which is characterized in that the dielectric substrate is silicon dioxide layer,
The thickness of the silicon dioxide layer is between 1 micron to 200 microns.
7. microelectrode system according to claim 1 or 2, which is characterized in that the material of first, second electrode is
Metal sensitive material, the metal sensitive material are gold, platinum or silver.
8. microelectrode system according to claim 1 or 2, which is characterized in that the dielectric substrate be quartz, glass or
Silicon substrate of the person Jing Guo insulation processing.
9. a kind of electrochemical sensor, which is characterized in that the electrochemical sensor includes claim 1 to 8 any one of them
Microelectrode system.
10. a kind of method preparing microelectrode system, including step：
The spin coating photoresist in clean dielectric substrate；
Photoetching is carried out to the photoresist of institute's spin coating, exposes microelectrode pattern；
Using sputtering or the method for vapor deposition, such as microelectrode described in any item of the claim 1 to 8 is formed on an insulating substrate
The microelectrode pattern of system；
Remove remaining photoresist.
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| CN201511021604.5A CN105651837B (en) | 2015-12-31 | 2015-12-31 | Microelectrode system and preparation method thereof, electrochemical sensor |
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| CN105651837B true CN105651837B (en) | 2018-10-23 |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN205844251U (en) * | 2016-07-20 | 2016-12-28 | 广州易活生物科技有限公司 | Detector electrode structure and detection orifice plate |
| CN107144744B (en) * | 2017-04-25 | 2018-07-20 | 云南大学 | A kind of electrode system measuring the electron transport performance in nanometer sized materials/structure |
| CN108414592A (en) * | 2018-02-05 | 2018-08-17 | 北京科技大学 | A kind of preparation method of polymer brush microelectrode array |
| CN109809359A (en) * | 2019-01-10 | 2019-05-28 | 北方工业大学 | 2.5D interdigital electrode manufacturing method and interdigital electrode |
| CN111122683A (en) * | 2019-12-12 | 2020-05-08 | 同济大学 | Electrochemical method for detecting cephalosporin by three-dimensional interdigital printed electrode |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN102326078A (en) * | 2009-01-09 | 2012-01-18 | 技术研究及发展基金有限公司 | Volatile organic compounds as diagnostic markers in the breath for lung cancer |
| CN102405409A (en) * | 2008-12-23 | 2012-04-04 | 3M创新有限公司 | Organic chemical sensor with microporous organosilicate material |
| CN102692439A (en) * | 2011-03-25 | 2012-09-26 | 中国科学院电子学研究所 | Microelectrode system having double-spiral structure, electrochemical sensor and preparation method of the microelectrode system having double-spiral structure |
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| WO2009106906A1 (en) * | 2008-02-27 | 2009-09-03 | Budapesti Müszaki És Gazdaságtudományi Egyetem | Interdigitated electrode |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102405409A (en) * | 2008-12-23 | 2012-04-04 | 3M创新有限公司 | Organic chemical sensor with microporous organosilicate material |
| CN102326078A (en) * | 2009-01-09 | 2012-01-18 | 技术研究及发展基金有限公司 | Volatile organic compounds as diagnostic markers in the breath for lung cancer |
| CN102692439A (en) * | 2011-03-25 | 2012-09-26 | 中国科学院电子学研究所 | Microelectrode system having double-spiral structure, electrochemical sensor and preparation method of the microelectrode system having double-spiral structure |
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